Impurity Removal Leading to High-Performance CoSb3‑Based Skutterudites with Synergistic Carrier Concentration Optimization and Thermal Conductivity Reduction

Li, Xu-Guang and Liu, Wei-Di and Li, Shuang-Ming and Li, Dou and Zhong, Hong and Chen, Zhi-Gang ORCID: https://orcid.org/0000-0002-9309-7993 (2021) Impurity Removal Leading to High-Performance CoSb3‑Based Skutterudites with Synergistic Carrier Concentration Optimization and Thermal Conductivity Reduction. ACS Applied Materials and Interfaces, 13 (45). pp. 54185-54193. ISSN 1944-8244


Abstract

Thermoelectric properties of CoSb3-based skutterudites are greatly determined by the removal of detrimental impurities, such as (Fe/Co)Sb2, (Fe/Co)Sb, and Sb. In this study, we use a facile temperature gradient zone melting (TGZM) method to synthesize high-performance CoSb3-based skutterudites by impurity removal. After removing metallic or semimetallic impurities (Fe/Co)Sb, (Fe/Co)Sb2, and Sb, the carrier concentration of TGZM-Ce0.75Fe3CoSb12 can be reduced to 1.21 × 1020 cm–3 and the electronic thermal conductivity dramatically reduced to 0.7 W m–1 K–1 at 693 K. Additionally, removing these impurities also effectively reduces the lattice thermal conductivity from 7.2 W m–1 K–1 of cast-Ce0.75Fe3CoSb12 to 1.02 W m–1 K–1 of TGZM-Ce0.75Fe3CoSb12 at 693 K. As a consequence, TGZM-Ce0.75Fe3CoSb12 approaches a high power factor of 11.7 μW cm–1 K–2 and low thermal conductivity of 1.72 W m–1 K–1 at 693 K, leading to a peak zT of 0.48 at 693 K, which is 10 times higher than that of cast-Ce0.75Fe3CoSb12. This study indicates that our facile TGZM method can effectively synthesize high-performance CoSb3-based skutterudites by impurity removal and set up a solid foundation for further development.


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Item Type: Article (Commonwealth Reporting Category C)
Refereed: Yes
Item Status: Live Archive
Additional Information: Files associated with this item cannot be displayed due to copyright restrictions.
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Date Deposited: 24 May 2022 03:54
Last Modified: 31 May 2022 02:07
Uncontrolled Keywords: thermoelectric; CoSb3; temperature gradient zone melting; synthesis; thermal conductivity
Fields of Research (2008): 10 Technology > 1007 Nanotechnology > 100708 Nanomaterials
09 Engineering > 0912 Materials Engineering > 091203 Compound Semiconductors
09 Engineering > 0912 Materials Engineering > 091205 Functional Materials
Fields of Research (2020): 40 ENGINEERING > 4016 Materials engineering > 401603 Compound semiconductors
40 ENGINEERING > 4016 Materials engineering > 401605 Functional materials
34 CHEMICAL SCIENCES > 3403 Macromolecular and materials chemistry > 340301 Inorganic materials (incl. nanomaterials)
40 ENGINEERING > 4018 Nanotechnology > 401807 Nanomaterials
Identification Number or DOI: https://doi.org/10.1021/acsami.1c16622
URI: http://eprints.usq.edu.au/id/eprint/48493

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